Biosorption of Lead (II) and Copper (II) from …absorbing lead (II) and copper (II) from aqueous...
Transcript of Biosorption of Lead (II) and Copper (II) from …absorbing lead (II) and copper (II) from aqueous...
Chiang Mai J. Sci. 2008; 35(1) 69
Biosorption of Lead (II) and Copper (II) from AqueousSolutionWoranart Jonglertjunya*Department of Chemical Engineering, Faculty of Engineering, Mahidol University, Bangkok, Thailand.
* Author for correspondence; e-mail: [email protected]
Received : 18 September 2007
Accepted : 5 October 2007
ABSTRACT
In this study, the potential of biosorption of heavy metal ions by corncob and the
natural fungi growing on corncob was investigated. Solutions containing lead (II) and copper
(II) ions were prepared synthetically in single component and the time required for attaining
biosorption equilibrium was studied. The effects of initial pH of heavy metal ions solutions
and biosorbent dosages in respective ranges of 4.0 to 6.0 and 150 to 350 g (wet weight) on
adsorption efficiency were also examined.Results showed the equilibrium time for biosorption
of lead and copper ions from the solution to be approximately 90 minutes. The optimum
initial pH for lead and copper adsorption by the natural fungi growing on corncob was 5.0.
Under these conditions, the biosorption of lead and copper ions solution was 4.29 and 1.76
mg metal/g dry biomass, respectively. When using corncob alone as control, the corresponding
values for the biosorption of lead and copper were 1.09 and 0.67 mg metal/g dry biomass,
respectively, at initial pH level of 5. The adsorption equilibrium data were adequately characterized
by both Langmuir and Freundlich equations. The maximum adsorption capacity based on the
Langmuir isotherm, was found to be 14.75 and 1.77 mg metal per g dry weight biosorbent
for lead and copper adsorption, respectively, at initial pH level of 5.0 by the natural fungi
growing on corncob.
Keywords: Biosorption, Wastewater Treatment, Heavy Metal Ions.
1. INTRODUCTION
Rapid industrialization has led to
increased disposal of wastewater into the
environment. This often exceeds the
admissible sanitary standards and results in the
adverse impact on aquatic environment and
consequently on human health. Wastewater
treatment has received greater attention over
the years due to the global awareness of the
environmental deterioration. However, the
application of various treatment techniques
needs to agree with the wastewater characteris-
tics. For example, the wastewater from food
and beverage industries mainly consists of high
organic compounds, which are commonly
found in microbiological treatment processes
such as activated sludge process. On the other
hand, metallurgical industry, electroplating and
metal finishing industries, tannery operations,
chemical manufacturing, mine drainage and
battery manufacturing are examples of the
Chiang Mai J. Sci. 2008; 35(1) : 69-81
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70 Chiang Mai J. Sci. 2008; 35(1)
industrial sources of heavy metals ions found
in wastewater. A variety of suitable methods
can be used for the removal of metal
pollutants from such liquid wastes, including
filtration, chemical precipitation, coagulation,
solvent extraction, electrolysis, ion exchange,
membrane process and adsorption. Ion
exchange and adsorption are the most
common and effective processes for the
removal of heavy metal ions [1]. However,
high operation cost and input of chemicals
often make these processes impractical and
result in further environment damage [2].
Treatment of effluents with heavy metals
following biotechnological approaches is
simple, comparatively inexpensive and friendly
to environment [2-4] Microbiological
processes are of significance in determining
metal mobility and have potential application
in bioremediation of metal pollution [5].
Bioleaching of heavy metals, biooxidation of
precious metal from ores, desulfurization of
coal and oil, and biosorption of metal ions
are examples of the wide variety of potential
applications of microorganisms in mining and
related fields [6, 7].
Biosorption is the uptake of heavy metal
and radionuclides from aqueous solution by
biological materials (i.e biosorbents) [8]. A
low cost sorbent is defined as one which is
abundant in nature, or is a by-product or waste
materials. Various waste biomaterials such as
grape stalk waste [1], green coconut shell
powder [9], chaff [2], and crab shell particles
[4] have been studied for the removal of heavy
metal ions from the effluents. In addition to
biomaterials, microorganisms have also been
used as metal sorbents. Bacteria, fungi, yeast
and algae have been reported to remove heavy
metals from aqueous solutions [10].
Fungi in particular have demonstrated
unique metal adsorption characteristics and are
easy to cultivate [11]. Living and dead cells of
fungi can be used for the removal of heavy
metal ions [12]. In related studies, metal
removal abilities of various species of fungi
have been investigated such as Phanerochaete
chrysosporium [13], Trametes versicolor [14],
Aspergillus niger [12], Phellinus badius [8], and
Aspergillus oryzae and Phizopus oryzae [11].
However, no previous study has reported the
application of natural fungi for wastewater
treatment purposes for heavy metal removal.
It is well recognized that natural fungi can be
easily grown in substantial amounts on
biomaterial waste. Thus, there is potential for
utilizing some vegetable wastes as alternative
low cost metal sorbents. Corncob is one of
such wastes generated in the community, which
has been satisfactorily used for growing natural
fungi. Therefore, a fungal biomass growing
on corncob could serve as an economical
means for the removal of metal ions from
aqueous solutions.
The objective of this study was to
investigate the potential of corncob and the
natural fungi growing on corncob for
absorbing lead (II) and copper (II) from
aqueous solution. Also the influence of
various parameters such as adsorption
equilibrium contact time, initial pH and
amount of biosorbent on adsorption potential
of corncob was studied in detail.
2. MATERIALS AND METHODS
2.1 Biosorbent Preparation
Yellow corn on the cob was boiled in
filtered water at 100°C for 30 minutes, and
then corn was removed from corncob. Boiled
corncob was next cut into cubical pieces of
about 1.3 centimeter. All experiments were
carried out in 1.5 liter round plastic drinking
bottles containing corncob. The gas supply
system was designed to accommodate
ambient air through cotton wool. Based on
the results obtained from cell dry weight of
the natural fungi growing on corncob, the
bottles were incubated outside the building
Chiang Mai J. Sci. 2008; 35(1) 71
under the shade for 7 days for optimal growth.
The control experiments were set up by
preparing a series of bottles with the same
composition with no fungi present.
2.2 Copper (II) and Lead (II) Solutions
The chemicals used for the study were
analytical grades lead nitrate (Pb(NO3)
2) and
copper sulphate (CuSO4) purchased locally
from BDH company, Bangkok. The copper
(II) and lead (II) solutions with concentration
of about 1000 mg/l were prepared by
dissolving the respective amounts in distilled
water. The exact heavy metal content of the
solutions was analyzed by an atomic
absorption spectrophotometer (AAS).
2.3 Equilibrium Contact Time
All experiments were carried out in 1.5
liter round plastic bottles containing 350 g (wet
weight) of corncob to serve as control.
Another identical plastic bottle contained
similar amount of corncob with fungi
growing on it naturally. Each bottle contained
0.5 liter of the copper (II) and lead (II)
solutions with concentration of about 1000
mg/l. The initial pH levels of heavy metal ions
solution were adjusted to 4.0, 5.0 and 6.0.
Duplicate trials were conducted in all tests. For
analysis, 5 ml sample was taken out from each
bottle at regular time intervals of 30, 60, 90,
120, and 150 minutes. The heavy metal ions
solution was passed through a filter paper
(Whatman No. 1) to separate solid and liquid
phases and the filtrate was used for analyzing
the copper and lead concentrations.
2.4 Effects of Initial pHs on Adsorption
Capacity
All experiments were conducted in
duplicate in a 1.5 liter round plastic bottles
containing 250 g (wet weight) of corncob
with and without natural growth of fungi.
Each bottle contained 0.5 liter of the copper
(II) and lead (II) solutions with concentration
of about 1000 mg/l. Three different level of
initial pH (4.0, 5.0 and 6.0) were maintained
in the solution. All samples were taken at
optimal equilibrium contact time and filtered
as described in previous section. The filtrate
was subsequently analyzed for copper and lead
concentrations. The solid part was dried at
60 oC until reaching a constant level and
recorded as dry weight.
The metal concentrations adsorbed on
the solid were calculated from the difference
between heavy metal ions content (in mg per
liter) in the liquid solution before (Ci) and after
adsorption (Ceq
). The following equations
were used to compute the adsorption
percentage (%Ad) and the absorption capacity
by the adsorbent, qeq
(mg metal per g dry
biosorbent), respectively:
100% ×⎥
⎦
⎤⎢⎣
⎡ −=
i
eqi
C
CCAd (1)
)
w
V)(CC(q eqieq −= (2)
where V (in liter) is the solution volume and
w (in gram) the amount of dry biosorbent
used.
2.5 Effects of Biosorbent Dosage on
Adsorption Capacity
The experimental procedure described
in the previous section was followed using
different amounts of corncob (150, 200, 250,
300 and 350 g wet weight) and optimal initial
pH level. The samples were taken out for
analysis at optimal equilibrium contact time.
The data was then used to compute %Ad,
and qeq
(mg metal per g dry biosorbent).
2.6 Analysis of the Copper (II) and Lead
(II) Concentration
Copper and lead contents in the solution
72 Chiang Mai J. Sci. 2008; 35(1)
were determined by an atomic absorption
spectrophotometer (AAS). Calibration curves
for each metal were determined using
standardized metal solutions. The solutions
were diluted with distilled water and later the
same day the amounts of copper and lead
were determined by AAS (3300 Perkin
Elmer).
3. RESULTS AND DISCUSSION
3.1 Equilibrium Contact Time
Adsorption equilibrium is defined as the
equilibrium distribution of a given component
between an adsorbate and adsorbent. The
equilibrium adsorption isotherm data can be
characterized by a model such as the Langmuir
equation.
meqm qbCqq
111+= (3)
where: q is the concentration of adsorbed
metal per unit weight of biosorbent, Ceq
is
the concentration of heavy metal ions in the
liquid phase, qm
is the maximum adsorption
capacity per unit weight of biosorbent and b
is the adsorption equilibrium constant.
Equilibrium data for the bacterial adsorption
is plotted as 1/q vs 1/Ceq
, according to the
Langmuir isotherm. The two constants qm
and
b are calculated from the slope (1/qmb) and
intercept (1/qm) of the line, respectively.
The equilibrium isotherm data can also
be characterized by a model such as the
Freundlich equation.
n/eqKCq 1
= (4)
where: K and n are empirical constants
indicative of sorption capacity and sorption
intensity, respectively. The Freundlich
parameters were obtained by fitting the
experimental data to the linearized equation
(plot of log q against log Ceq
).
Figures 1 and 2 show the results on the
adsorption of lead (II) and copper (II) ions
from the solutions, respectively, at three
different initial pH levels. The heavy metal ions
concentration in the liquid-phase decreased
rapidly with time apparently due to the
adsorption of metal ions on the corncob and
finally leveled off. The results presented in
Figures 1 and 2 also showed that the amount
of adsorbed heavy metal ions was dependent
on the initial pH of the solution and the type
of biosorption media.
The initial sharp decrease in heavy metal
ions concentration in the liquid-phase implied
higher rate of biosorption (Figures 1 and 2).
The rate of biosorption was markedly
influenced by the levels of initial pH in the
solution. The overall results indicated that
the adsorption of heavy metal ions was
comparatively higher at initial pH of 5.0
irrespective of the presence of fungi on
corncob. The biosorption by the natural fungi
growing on corncob showed similar patterns
to corncob without fungal growth. The
reduction in heavy metal ion concentration in
the liquid phase resulting from the natural fungi
growing on corncob (Figures 1(b) and 2(b))
was much greater than the control experiments
(Figures 1(a) and 2 (a)). The adsorption of
heavy metal ions was enhanced by the
filamentous fungi present on the corncob
surfaces.
Adsorption of lead (II) and copper (II)
on corncob reached equilibrium levels both
in presence of natural fungal growth and
control samples as shown in Figures 1 and
2. Apparently, equilibrium adsorption levels
were attained after about 90 minutes of
exposure for all pH levels investigated in this
study. The data beyond 90 minutes indicated
only a little adsorption. The equilibrium
adsorption trends of copper (II) were in
good agreement with those of lead (II)
solution. The short equilibrium adsorption
contact time of about 90 minutes in lead (II)
Chiang Mai J. Sci. 2008; 35(1) 73
and copper (II) ions solutions in general agreed
with the other findings [4,14,15]. Taking into
account these results, a contact time of 90
minutes was chosen for further experiments
irrespective of initial pH level.
Figure 1. Biosorption of lead (II) ions as a function of time for (a) corncob alone and (b) in
the presence of natural fungi growing on corncob.
Figure 2. Biosorption of copper (II) ions as a function of time for (a) corncob alone and (b)
in the presence of natural fungi growing on corncob.
74 Chiang Mai J. Sci. 2008; 35(1)
3.2 Effects of initial pHs on adsorption
capacity
The pH of metal solution has been
identified as one of the most important
variables governing the biosorption process.
Based on the finding of optimum pH levels
in several studies [1,8,12-14,16] the range of
pH selected in this study was between 4
and 6.
The absorption capacity and the
adsorption percentage of lead (II) and copper
(II) ions solutions for different initial pH levels
are shown in Figures 3 and 4, respectively.
The adsorption capacity of lead (II) ions in
case of control corncob sample
(Figure 3) increased slightly with
increasing initial pH from 0.8 to 1.3 mg metal
per g dry weight biosorbent with
corresponding adsorption percentage ranging
from 23 to 38, respectively. The adsorption
capacity of lead (II) ions by the natural fungi
growing on corncob was relatively higher in
the range of 2.0 to 2.6 mg metal per g dry
weight biosorbent corresponding to the
adsorption percentage of about 67 to 77,
respectively. The optimum initial pH for lead
adsorption by the natural fungi growing on
corncob was found to be 5.0.
Figure 3. Comparison of the absorption capacity (q) and the adsorption percentage (%Ad)
of lead (II) ions by corncob alone and in the presence of natural fungi growing on
corncob for different initial pH levels.
The adsorption capacity of lead (II) ions
solution in the presence of fungi was much
greater than the control experiments. The
natural fungi growing on corncob at initial pH
5 resulted in the maximum adsorption capacity
of 2.6 mg metal per g dry weight biosorbent
in lead (II) solution as compared to about 0.9
mg metal per g dry weight biosorbent by the
corncob alone. This clearly demonstrated that
an increase in the adsorption capacity of lead
(II) ions because of the influence of fungi.
As shown in Figure 4, no significant
Chiang Mai J. Sci. 2008; 35(1) 75
difference was found in the values of the
absorption capacity and percentage in case of
copper (II) ions solution by corncob. The
adsorption capacity in copper (II) ions solution
was found to be about 0.6, 0.6 and 0.7 mg
metal per g dry weight biosorbent
corresponding to the same adsorption
percentage of about 19 for initial pH level of
4.0, 5.0 and 6.0, respectively. Although the
effect of initial pH on metal adsorption in
the control experiments was not significantly
different, it had a noticeable effect in the
presence of the natural fungi growing on
corncob. The corncob with fungi showed
adsorption capacity of copper (II) ions to be
1.0, 1.2 and 0.7 mg metal per g dry weight
biosorbent corresponding to the adsorption
percentage of about 34, 38 and 24 for initial
pH of 4.0, 5.0 and 6.0, respectively. Thus,
the optimum initial pH of 5.0 for copper
adsorption by the natural fungi growing on
corncob was found to be similar to the case
of lead (II) adsorption.
Overall results indicated the adsorption
capacity of copper (II) ions solution to be
very low in comparison to that of lead (II)
adsorption experiments in case of both
biosorbents. This may be probably due to the
difference in natural affinity between the type
of heavy metal and biosorbent. A direct
comparison of these findings is not possible
with the values reported in literature due to
different study conditions, metal ions and
fungus strains used in various studies.
However, the results on the adsorption of
lead (II) and copper (II) ions are in agreement
with the previous studies [12,14] by the live
cells showing comparatively higher adsorption
of lead (II) ions from the solution.
3.3 Effects of biosorbent dosage on
adsorption capacity
Biosorbent dosages may have a
significant influence on the adsorption capacity
and percentage. Vijayaraghavan et al. [4] found
that the percentage of copper and cobalt
removal by crab shell particles increased with
increase in biosorbent dosage, however,
biosorption efficiency (mg metal per g
biosorbent) decreased with increase in
biosorbent dosage. The small number of
published papers available does not allow
researchers to draw a sound conclusion; the
present study may contribute to fill this
apparent gap in knowledge.
Figure 4. Comparison of the absorption
capacity (q) and the adsorption
percentage (%Ad) of copper (II)
ions by corncob alone and in the
presence of natural fungi growing
on corncob for different initial pH
levels.
76 Chiang Mai J. Sci. 2008; 35(1)
Figure 5. Comparison of the absorption capacity (q) and the adsorption percentage (%Ad)
of lead (II) ions by corncob alone and in the presence of natural fungi growing on
corncob for different biosorbent dosages.
Figures 5 and 6 present typical set of
results obtained by varying biosorbent
dosages from 150 to 350 g (wet weight)
during lead and copper biosorption,
respectively. The adsorption of lead (II) ions
by the corncob (Figure 5) showed only a little
change in the value of q ranging from 1.23 to
0.78 mg metal per g dry weight biosorbent.
In addition, the percentage adsorption of lead
(II) ions by the corncob increased from about
20 to 44 % when the biosorbent dosage was
increased from 150 to 350 g.
In contrast, the adsorption of lead (II)
ions by the natural fungi growing on corncob
as shown in Figure 5 was markedly decreased
from 4.3 to 2.0 mg metal per g dry weight
biosorbent with an increase in biosorbent
dosage from 150 to 350 g. However, an
increase in the adsorption percentage of lead
(II) absorption from about 75 to 84 % by the
natural fungi growing on corncob appeared
to be gradual with a corresponding increase
in biosorbent dosage from 150 to 350 g.
The changes in the adsorption of copper
(II) ions followed the trends similar to lead
(II) ions as shown in Figure 6. The absorption
capacity of copper (II) ions by corncob alone
indicated a mean value of about 0.64 mg
metal per g dry weight biosorbent for two
replications and different dosages of
biosorbent. However, there was a decrease
in the absorption capacities of copper (II) ions
in case of the natural fungi growing on
corncob when biosorbent dosage increased
from 150 to 350 g. For 150 g of corncob
with the natural fungi, there was approximately
a two-fold decrease in the copper adsorption
as compared to 350 g of the same biosorbent.
Chiang Mai J. Sci. 2008; 35(1) 77
Figure 6. Comparison of the absorption capacity (q) and the adsorption percentage (% Ad)
of copper (II) ions by corncob alone and in the presence of natural fungi growing
on corncob for different biosorbent dosages
An increase in adsorption percentage was
observed in both experiments. The
adsorption percentage increased from 12 to
28 % for corncob used as control and from
27 to 43 % for the natural fungi growing on
corncob. These results are in good agreement
with Vijayaraghavan et al. [4] who reported
overall similar trends in an increase in the
adsorption percentage with increasing
biosorbent dosage despite the different type
of biosorbent. The highest adsorption
percentage of about 43 % was achieved for
350 g of corncob with natural fungal growth.
In general, the absorption capacity and
the adsorption percentage for copper (II)
solution were much lower than those of lead
(II) solution. This was an approximately two-
fold decrease in the copper adsorption
compared to the lead adsorption. Again, the
nature of biosorbent particles might have
played an important role in the adsorption
of different metal ions.
The equilibrium adsorption isotherms
data for lead and copper by the natural fungi
growing on corncob at initial pH of 5.0 are
characterized in Figures 7 and 8, respectively,
based on Equations 3 and 4 when the
biosorbent dosage varied between 150 and
350 g. For each biosorbent dosage, the
concentration of adsorbed metal per unit
weight of biosorbent (q) and the
concentration of heavy metal ions in the liquid
phase (Ceq
) were determined for equilibrium
time of 90 minutes. The equilibrium data for
78 Chiang Mai J. Sci. 2008; 35(1)
the lead adsorption was plotted as 1/q vs 1/
Ceq
, and log q vs log C
eq, according to
Equations 3 and 4, respectively. Subsequently,
the equation parameters for Langmuir
equation (qm and b) and Freundlich equation
(K and n) were determined from the slope
and intercept of the least-squares fits. Similar
analysis was carried out to determine
parameters (qm, b, K and n) for copper
adsorption from the plots of equilibrium data
as shown in Figure 8.
Figure 7. Plots for determining the parameters of Langmuir and Freundlich equations for
the adsorption of lead (II) ions by natural fungi growing on corncob (solution pH
5.0).
Figure 8 .Plots for determining the parameters of Langmuir and Freundlich equations for
the adsorption of copper (II) ions by the natural fungi growing on corncob (solution
pH 5.0).
Table 1 presents the results of regression
analysis for determining the parameters of
Langmuir and Freundlich equations (Equations
3 and 4). The coefficient of determination
(R2) ranged from 0.70 to 0.74 and 0.88 to
0.91 for adsorption of lead and copper,
respectively. These results indicated that the
equilibrium adsorption data of lead and
copper conformed reasonably well to the
Langmuir and Freundlich equations. Table 2
presents a general comparison of the results
of this study with other published work for
adsorption of lead and copper by different
fungal species. In particular, there is reasonable
agreement with the work of Kapoor et al.
[12] and Yetis et al. [13] Yan and Viraraghavan
[16 ].
Chiang Mai J. Sci. 2008; 35(1) 79
Table 1. Regression parameters of Langmuir and Freundlich equations for biosorption of
lead and copper by the natural fungi growing on corncob at initial pH of 5.0.
Langmuir equation Freundlich equation
Metal qm (mg metal K (mg metal per g
adsorption per g dry b R2 dry weight n R2
weight biosorbent)
biosorbent)
lead 14.75 7.03 x 10 -4 0.7417 2.39 x 10 -3 0.77 0.7037
copper 1.77 6.92 x 10 -4 0.8816 2.40 x 10 -5 0.59 0.9107
Table 2. Comparison of the parameters of Langmuir and Freundlich equations reported in
literature.
Langmuir equation Freundlich equation
References Adsorbent Heavy
metal qm
b R2 K n R2
ions
[1] Aspergillus niger Pb 598.0 4x10-4 0.61 0.63 0.6 0.62
(Live cell)
NaOH pretreated Pb 10.19 7.8 0.81 8.27 7.19 0.97
Aspergillus niger
pH = 5 Cu 4.69 0.30 0.88 1.47 0.79 0.79
[14] Immobilized Trametes Pb 194.76 6.13x10-4 0.98 190.61 3.16 0.945
versicolor
(Live cell) Cu 104.85 6.11x10-4 0.908 45.12 2.98 0.984
[16] Mucor rouxii Pb 35.69 0.80 0.95 14.31 2.10 0.88
(Live cell)
Mucor rouxii Pb 25.22 0.87 0.86 10.73 2.50 0.80
(dead cell)
[8] Phellinus badius Pb 169.90 6.07 0.997 - - -
(Live cell)
[13] Phanerochaete
chrysosporium Pb 33.00 0.01 0.03 5.47 8.31 0.09
(Live cell)
This work The natural fungi Pb 14.75 7.03 x 10-4 0.74 2.39 x 10-3 0.77 0.70
growing on corncob
Cu 1.77 6.92 x 10-4 0.88 2.40 x 10-5 0.59 0.91
80 Chiang Mai J. Sci. 2008; 35(1)
The parameters in Langmuir and
Freundlich equations (qm, b, K and n) have
been reported to depend on several factors
such as the experimental conditions, types of
metal ions and fungus strains used as
biosorbents. Specifically, the values of both
qm
and K in case of lead adsorption were
significantly higher than in copper adsorption,
which agrees with the findings of other
researchers. Also the decrease in the values of
qm and K for copper adsorption could be
explained by the lower affinity due to the
nature of biosorbent.
4. CONCLUSION
Adsorption of lead (II) and copper (II)
in the presence of natural fungi growing on
corncob attained equilibrium after about 90
minutes of exposure for initial pH ranging
from 4.0 to 6.0. The optimum pH level for
lead and copper adsorption by the natural
fungi growing on corncob was found to be
5.0. The overall adsorption percentage
increased with an increase in the biosorbent
dosage, but the biosorption efficiency (mg
metal per g biosorbent) was decreased.
Results showed maximum adsorption
capacity per unit dry weight of biosorbent
based on Langmuir isotherm to be 14.75 and
1.77 mg metal per g dry weight biosorbent
for lead and copper adsorption, respectively,
by the natural fungi growing on corncob.
ACKNOWLEDGEMENTS
I wish to thank the Faculty of
Engineering, Mahidol University for the
project grant. This work was supported by
the equipment in the Department of Chemical
Engineering, the Faculty of Engineering,
Mahidol University.
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